The high purity crystal of 2,4-dinitrotoluene (DNT) could be successfully recovered from spent acid in a short period through diluting method assisted with ultrasonic irradiation. The sonication tests were carried out to elucidate the influence of various ultrasonic powers on the performance of crystallization of 2,4-DNT. It is remarkable that under the supersaturated condition ultrasonic irradiation could significantly accelerate the crystal formation, in which the purity of 2,4-DNT reaches to approximate 98.9 wt%. Based on the particle size distribution of crystals, it is proposed that the enhancement on recovery rate of 2,4-DNT crystals by ultrasound is mainly ascribed to the elevation of mass transfer rate for crystal growth. According to the spectra examined by field emission scanning electron microscope (FESEM), the above hypothesis is further verified by the appearance of smoother surface of crystals. Furthermore, the results of metallurgical microscope measurements show that ultrasound has also an abrasive effect on 2,4-DNT crystals under high ultrasonic power inputs.